The assertion of intrinsic material properties based on measured experimental data is being challenged by emerging sample synthesis protocols, which opens new avenues for discovering novel functionalities. In this study, we revisit one of the most widely studied strongly correlated materials of the early 2000s, NaxCoO2 (NCO). Leveraging the sensitivity of muon spin rotation and relaxation (μ+SR) measurements, we discern significant differences between NCO samples synthesized via conventional solid-state reaction (SSR) and our electrochemical reaction (ECR) approach. Contrary to SSR-synthesized Na0.7CoO2, which exhibits a nonmagnetic ground state, our ECR-derived sample showcases an antiferromagnetic (AF) order from x≥0.7, challenging established phase boundaries. We attribute the observed magnetic phenomena in ECR-NCO to long-range order of Na-ions and/or vacancies, as well as the inherent flexibility of the crystal framework. Our study holds implications for tailoring and optimization of next-generation devices based on layered materials.

In this study, we investigate the influence of Cr-Cr distances on the magnetic properties of triangular lattice antiferromagnets through the lens of the recently synthesized Cr compounds LiCrSe2, 2 , LiCrTe2, 2 , and NaCrTe2. 2 . Our comprehensive analysis integrates existing magnetic structure data and new insights from muon spin rotation measurements, revealing a striking mutual influence between strongly correlated electrons and structural degrees of freedom in systems possessing very different magnetic properties despite having the same crystal symmetry. In particular, we delineate how Cr-Cr distances specifically dictate the magnetic behaviors of the triangular lattice antiferromagnets LiCrSe2, 2 , LiCrTe2, 2 , and NaCrTe2. 2 . By crafting phase diagrams based on these distances, we establish a clear correlation between the structural parameters and the magnetic ground states of these materials together with a wide variety of trivalent Cr triangular lattice layered magnets. Our analysis uncovers a transition range for in-plane and out-of-plane Cr-Cr distances that demarcates distinct magnetic behaviors, highlighting the nuanced role of lattice geometry in the spin-lattice interaction and electron correlation dynamics.

A Muon Spin Rotation (mu+SR) study was conducted to investigate the magnetic properties of SrCu2(BO3)(2) (SCBO) as a function of temperature/pressure. Measurements in zero field and transverse field confirm the absence of long range magnetic order at high pressures and low temperatures. These measurements suggest changes in the Cu spin fluctuations characteristics above 21 kbar, consistent with the formation of a plaquette phase as previously suggested by inelastic neutron scattering measurements. SCBO is the only known realisation of the Shatry-Sutherland model, thus the ground state mediating the dimer and antiferromagnetic phase is likekly to be a plaquette state.

LiFePO4 (LFPO) is an archetypical and well-known cathode material for rechargeable Li-ion batteries. However, its quasi-one-dimensional (Q1D) structure along with the Fe ions, LFPO also displays interesting low-temperature magnetic properties. Our team has previously utilized the muon spin rotation (mu+SR) technique to investigate both magnetic spin order as well as Li-ion diffusion in LFPO. In this initial study we extend our investigation and make use of high-pressure mu+SR to investigate effects on the low-T magnetic order. Contrary to theoretical predictions we find that the magnetic ordering temperature as well as the ordered magnetic moment increase at high pressure (compressive strain).

In an all solid state Li-ion battery, it is crucial to reduce ionic resistivity at the interface between the electrode and the electrolyte in order to enhance Li+ mobility across the interface. Recent first principles calculations predict the presence of a space-charge layer (SCL) at the interface due to the difference in the Li+ chemical potential at the interface between two different materials, as in the metal-semiconductor junction in electronic devices. However, the presence of SCL has never been experimentally observed. Our first attempt in a fresh multilayer sample, Cu(10 nm)/Li3PO4(50 nm)/LiCoO2(100 nm) on a sapphire substrate, with low-energy mu+SR (LE mu+SR) revealed a gradual change in the nuclear magnetic field distribution width as a function of implantation depth even across the interface between Li3PO4 and LiCoO2. This implies that the change in the field distribution width at SCL of the sample is too small to be detected by LE mu+SR.

The internal magnetic field in a ferromagnetic compound, Y2Co12P7 with T-C = 150 K, was studied with mu(+) SR using a powder sample down to 2 K. The wTF-mu(+) SR measurements revealed the presence of a sharp magnetic transition at T-C = 151 K, and the ZF-mu(+) SR measurements clarified the formation of static magnetic order below T-C. The presence of two muon spin precession signals in the ZF-mu(+) SR spectrum below TC indicates the existence of the two different muon sites in the lattice. By considering the muon sites and local spin densities at the muon sites predicted with DFT calculations, the ordered magnetic moments of Co were successfully determined.

The diffusive behavior in a spinel-type Li+ ion battery material, Li[Ni1/2Mn3/2]O4, has been studied with positive and negative muon spin rotation and relaxation (μ±SR) measurements in the temperature range between 200 and 400 K using a powder sample. The implanted μ+ locates at an interstitial site near O2- ion so as to form a O-H like bond, while the implanted μ- is mainly captured by an oxygen nucleus, resulting in the formation of muonic oxygen. This means that local magnetic environments in Li[Ni1/2Mn3/2]O4 were investigated from the two different sites in the lattice, i.e., one is an interstitial site for μ+SR and the other is an oxygen site for μ-SR. Since both μ+SR and μ-SR detected an increase in the fluctuation rate of a nuclear magnetic field for temperatures above 200 K, the origin of this increase is clearly confirmed as Li diffusion. Assuming a random walk process with the hopping of thermally activated Li+ between a regular Li site and the nearest neighboring vacant octahedral sites, a self-diffusion coefficient of Li+ was found to range above 10-11 cm2/s at temperatures above 250 K with an activation energy of about 0.06 eV.

The influence on the decomposition and reforming of the hydrogen storage material NaAlH₄ by adding relatively low amounts of mesoporous carbon black is investigated with in situ diffraction. A 60:40 NaAlH₄/carbon black composite is prepared via ball milling and characterised ex situ via X-ray diffraction, gas adsorption, temperature-programmed decomposition, and dehydrogenation/hydrogenation cycling methods. The prepared composite is deuterated, and the crystalline phase composition is determined with in situ neutron powder diffraction method during multiple decomposition/deuteration cycles. Changes in the crystalline phase composition start slightly below the melting temperature of the pristine alanate, whereas the release of deuterium starts at considerably lower temperatures. The decomposition of Na₃AlD₆ to NaD is almost completely reversible at the applied low deuterium pressures of >= 2 MPa. Thus, the strong effect of even low concen-trations of a mesoporous carbon black on the capability to store H₂ reversibly is showcased and analysed in-depth.

The magnetism of double perovskites is a complex phenomenon, determined from intra- or interatomic magnetic moment interactions, and strongly influenced by geometry. We take advantage of the complementary length and timescales of the muon spin rotation, relaxation, and resonance (mu+SR) microscopic technique and bulk ac/dc magnetic susceptibility measurements to study the magnetic phases of the LaCaNiReO6 double perovskite. As a result, we are able to discern and report ferrimagnetic ordering below TC = 102 K and the formation of different magnetic domains above TC. Between TC < T < 270 K, the following two magnetic environments appear, a dense spin region and a static-dilute spin region. The paramagnetic state is obtained only above T > 270 K. An evolution of the interaction between Ni and Re magnetic sublattices, in this geometrically frustrated fcc perovskite structure, is revealed as a function of temperature through the critical behavior and thermal evolution of microscopic and macroscopic physical quantities.

Two-dimensional (2D) triangular lattice antiferromagnets (2D-TLA) often manifest intriguing physical and technological properties, due to the strong interplay between lattice geometry and electronic properties. The recently synthesized 2-dimensional transition metal dichalcogenide LiCrTe2, being a 2D-TLA, enriched the range of materials which can present such properties. In this work, muon spin rotation (μ+SR) and neutron powder diffraction (NPD) have been utilized to reveal the true magnetic nature and ground state of LiCrTe2. From high-resolution NPD the magnetic spin order at base-temperature is not, as previously suggested, helical, but rather collinear antiferromagnetic (AFM) with ferromagnetic (FM) spin coupling within the ab-plane and AFM coupling along the c-axis. The value if the ordered magnetic Cr moment is established as μCr=2.36μB. From detailed μ+SR measurements we observe an AFM ordering temperature TN≈ 125 K. This value is remarkably higher than the one previously reported by magnetic bulk measurements. From μ+SR we are able to extract the magnetic order parameter, whose critical exponent allows us to categorize LiCrTe2 in the 3D Heisenberg AFM universality class. Finally, by combining our magnetic studies with high-resolution synchrotron X-ray diffraction (XRD), we find a clear coupling between the nuclear and magnetic spin lattices. This suggests the possibility for a strong magnon–phonon coupling, similar to what has been previously observed in the closely related compound LiCrO2.